Two of the major problems in using meteorological models to explain observed tropospheric trace constituent distributions and thereby to understand the global budgets of the tracers are to properly define the vertical layered structure in the free atmosphere, and to understand the contribution of advection processes in generating horizontal inhomogeneities at all scales. We proposed to tackle these problems through the examination of an extensive collection of trace constituent data from research and commercial aircraft in conjunction with meteorological data from the European Center for Medium-Range Weather Forecasts. The physical mechanisms responsible for these advection and layering processes were explored and their implications for theories and models assessed. In addition, we calculated examples of how thin layers (not currently resolved by models) affect the radiative heating/cooling rates. We developed an improved algorithm for trace constituent layer detection, and used it to analyze over 100,000 km of ozone and humidity vertical profiles collected by instruments piggybacked on commercial aircraft. The same method was also used to examine ozone, humidity, carbon monoxide, and methane data from the NASA Pacific Exploratory Missions. The major conclusions from these studies were that tropospheric trace constituent layers are ubiquitous, and that their characteristics are remarkably universal. These results support the notion that ozone layers coming in from the stratosphere play a large role in creating tropospheric layers, whether by themselves or by capping buoyant pollution plumes. This, in turn, has important implications for the transport (especially in the vertical) of trace gases and how it is represented in models.